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Discontinuous shear thickening (DST) is associated with a sharp rise in a suspension’s viscosity with increasing applied shear rate or stress. Key signatures of DST, highlighted in recent studies, are the very large fluctuations of the measured stress as the suspension thickens with increasing rate. A clear link between microstructural development and the dramatic increase in stress fluctuations has not been established yet. To identify the microstructural underpinnings of this behavior, we perform simulations of sheared dense suspensions. Through an analysis of the particle contact network, we identify a subset of constrained particles that contributes directly to the rapid rise in viscosity and large stress fluctuations. Indeed, both phenomena can be explained by the growth and percolation of constrained particle networks—in direct analogy to rigidity percolation. A finite size scaling analysis confirms this to be a percolation phenomenon and allows us to estimate the critical exponents. Our findings reveal the specific microstructural self-organization transition that underlies DST. 

Monodisperse suspensions of Brownian colloidal spheres crystallize at high densities, and ordering under shear has been observed at densities below the crystallization threshold. We perform large-scale simulations of a model suspension containing over [Formula: see text] particles to quantitatively study the ordering under shear and to investigate its link to the rheological properties of the suspension. We find that at high rates, for [Formula: see text], the shear flow induces an ordering transition that significantly decreases the measured viscosity. This ordering is analyzed in terms of the development of layering and planar order, and we determine that particles are packed into hexagonal crystal layers (with numerous defects) that slide past each other. By computing local [Formula: see text] and [Formula: see text] order parameters, we determine that the defects correspond to chains of particles in a squarelike lattice. We compute the individual particle contributions to the stress tensor and discover that the largest contributors to the shear stress are primarily located in these lower density, defect regions. The defect structure enables the formation of compressed chains of particles to resist the shear, but these chains are transient and short-lived. The inclusion of a contact friction force allows the stress-bearing structures to grow into a system-spanning network, thereby disrupting the order and drastically increasing the suspension viscosity.